In this article, the scattering of surface plasmon polaritons (SPPs) into photons at holes is investigated. A local, electrically excited source of SPPs using a scanning tunnelling microscope (STM) produces an outgoing circular plasmon wave on a thick (200 nm) gold film on glass containing holes of 250, 500 and 1000 nm diameter. Fourier plane images of the photons from hole-scattered plasmons show that the larger the hole diameter, the more directional the scattered radiation. These results are confirmed by a model where the hole is considered as a distribution of horizontal dipoles whose relative amplitudes, directions, and phases depend linearly on the local SPP electric field. An SPP-Young's experiment is also performed, where the STM-excited SPP-wave is incident on a pair of 1 $μ$m diameter holes in the thick gold film. The visibility of the resulting fringes in the Fourier plane is analyzed to show that the polarization of the electric field is maintained when SPPs scatter into photons. From this SPP-Young's experiment, an upper bound of $\approx$ 200 nm for the radius of this STM-excited source of surface plasmon polaritons is determined.
Correlated polarization dependences between surface-enhanced resonant Raman scattering and plasmon resonance elastic scattering showing spectral uncorrelation to each other
Surface plasmon polaritons scattering from 2D subwavelength silicon wires is investigated using finite difference time domain method. It is shown that coupling an incident surface plasmon polariton to inter-cavity modes of the particle can dramatically changes transmitted fields and plasmon induced forces. In particular, both transmission and optical forces are highly sensitive to the particle size that is related to the excitation of whispering gallery modes or standing-wave modes depending on the particle shape and size. This features might have potential sensing applications.
The ability to control propagation of electromagnetic guided modes lies at the heart of integrated nanophotonics. Surface plasmon-polaritons are a class of guided modes which can be employed in integrated optical systems. Here, we present a theoretical design of a coherent surface plasmon absorber which can perfectly harvest energy of coherently incident surface plasmons without parasitic scattering into free space modes. Excitation of free space modes which usually accompanies scattering of a surface plasmon by an interface boundary is avoided due to specially tailored anisotropy of the absor…
Nanosphere-on-mirror plasmonic antennas, each having a monolayer graphene or MoS2 sheet in the gap, were pumped with a femtosecond laser. Abrupt turnings in the scattering linewidth and peak intensity trends as the laser power changed were experimentally observed. Theoretical modelling of dynamic plasmon evolvement attributes the turning to transitioning between two plasmon states, with a universal switching threshold of four-wave mixing efficiency around 0.14%. This bistability is rendered by a strong feedback from the nonlinear gap current to the gap plasmons, and involvement of both four an…
High-energy (1-100 keV) electrons can coherently couple to plasmonic and dielectric nanostructures creating cathodoluminescence (CL) of which the spectral features reveal details of the material's resonant modes at deep-subwavelength spatial resolution. While CL provides fundamental insight in optical modes, detecting its phase has remained elusive. Here, we introduce Fourier-transform CL holography as a method to determine the far-field phase distribution of scattered plasmonic fields. We record far-field interferences between a transition radiation reference field and surface plasmons scatte…
A matrix balanced version of the Recursive Centered T Matrix Algorithm (RCTMA) applicable to systems possessing resonant inter-particle couplings is presented. Possible domains of application include systems containing interacting localized plasmon resonances, surface resonances, and photonic jet phenomena. This method is of particular interest when considering modifications to complex systems. The numerical accuracy of this technique is demonstrated in a study of particles with strongly interacting localized plasmon resonances.
Bio-compatible Au nanoparticles exhibit great advantages in the application of biomedical researches, such as bio-sensing, medical diagnosis, and cancer therapy. Bio-molecules can even be manipulated by laser tweezers with the optically trapped Au nanoparticles as handles. In this Letter, optical scattering torque arising from the coupled Au nanoparticles driven by circularly polarized light is theoretically presented. The coupled plasmon resonance modes boost the angular momentum transfer from photons to the Au nanoparticle dimers and trimers through light scattering, which does not bring any…
Scattering properties of a single plasm on interacting with three non-equally spaced quantum dots coupled to one-dimensional surface plasmonic waveguide is investigated theoretically via the real-space approach. It is demonstrated that the transmission and reflection of a single plasmon can be switched on or off by controlling the detuning and changing the interparticle distances between the quantum dots. By controlling the transition frequencies and interparticle distances of QDs, one can construct a half-transmitting mirror with three QDs system. We also showed that controlling the transitio…
We demonstrate importance of molecular multiple excitons and higher-order plasmons for both enhancement and quenching of resonance Raman and fluorescence of single dye molecule located at plasmonic hotspot under strong coupling regime. The multiple excitons induce complicated spectral changes in plasmon resonance and higher-order plasmons yield drastic quenching for both resonant Raman and fluorescence. A coupled oscillator model composed of plasmon and multiple excitons reproduces the complicated spectral changes. Purcell factors derived from higher-order plasmons reproduce the drastic quench…
Light scattering by small particles has a long and interesting history in physics. Nonetheless, it continues to surprise with new insights and applications. This includes new discoveries, such as novel plasmonic effects, as well as exciting theoretical and experimental developments such as optical trapping, anomalous light scattering, optical tweezers, nano-spasers, and novel aspects and realizations of Fano resonances. These have led to important new applications, including several ones in the biomedical area and in sensing techniques at the single-molecule level. There are additionally many …
The longitudinal and the transverse beam shifts, namely, the Goos-Hänchen (GH) and the Spin-Hall (SH) shifts are usually observed at planar interfaces. It has recently been shown that the transverse SH shift may also arise due to scattering of plane waves. Here, we show that analogous in-plane (longitudinal) shift also exist in scattering of plane waves from micro/nano systems. We study both the GH and the SH shifts in plasmonic metal nanoparticles/ nanostructures and dielectric micro-particles employing a unified framework that utilizes the transverse components of the Poynting vector of the …
Recently, guiding electromagnetic surface waves without sacrificing scattering losses through paths that have arbitrary shape bumps has gained a lot of interest due to its wealth of advantages in modern photonics and plasmonics devices. In this study, based on transformation optics (TO) methodology, a feasible approach to control the flow of surface plasmon plariton (SPPs) at metal-dielectric interfaces with arbitrary curvature is proposed. The obtained material becomes homogeneous and independent of the bump's geometry. That is, one constant material is required to route SPP waves without sca…
Molecular vibrations and their dynamics are of outstanding importance for electronic and thermal transport in nanoscale devices as well as for molecular catalysis. The vibrational dynamics of <100 molecules are studied through three-colour time-resolved coherent anti-Stokes Raman spectroscopy (trCARS) using plasmonic nanoantennas. This isolates molecular signals from four-wave mixing (FWM), while using exceptionally low nanowatt powers to avoid molecular damage via single-photon lock-in detection. FWM is found to be strongly suppressed in nm-wide plasmonic gaps compared to plasmonic nanopartic…
Plasmonic antennas integrated on silicon devices have large and yet unexplored potential for controlling and routing light signals. Here, we present theoretical calculations of a hybrid silicon-metallic system in which a single gold nanoantenna embedded in a single-mode silicon waveguide acts as a resonance-driven filter. As a consequence of scattering and interference, when the resonance condition of the antenna is met, the transmission drops by 85% in the resonant frequency band. Firstly, we study analytically the interaction between the propagating mode and the antenna by including radiativ…
We analyze the scattering of the surface plasmon incident at a planar interface between two dielectrics. By using the scattering matrix technique, developed by Oulton et al. [Phys. Rev. B 76, 035408 (2007)], we calculate the transmission, reflection coefficients and radiative losses for oblique incident angles. We found that the transmission of a surface wave through a single interface between two dielectrics may be accompanied with radiation losses of 10-40 per cent of the plasmon energy.
We show that the scattering interaction between a high energy electron and a photon can be strongly enhanced by different types of localized plasmons in a non-trivial way. The scattering interaction is predicted by an eigen-response theory, numerically verified by finite-difference-time-domain simulation, and experimentally verified by cathodoluminescence spectroscopy. We find that the scattering interaction associated with dark plasmons can be as strong as that of bright plasmons. Such a strong interaction may offer new opportunities to improve single-plasmon detection and high-resolution cha…
Surface enhanced Raman scattering mediated by surface plasmons polaritons with wave vector much larger than those of light is considered. The excitation of these polaritons and their efficient Raman scattering due to low group velocity and electric field localization at the surface is discussed for the case of two nearby surfaces. The Raman scattering depends not only on the intensity of the electric fields seen by the molecules but also on the surface plasmon density of states.
We report plasmon-enhanced Raman scattering in graphene coupled to a single plasmonic hotspot measured as a function of laser energy. The enhancement profiles of the G peak show strong enhancement (up to $10^5$) and narrow resonances (30 meV) that are induced by the localized surface plasmon of a gold nanodimer. We observe the evolution of defect-mode scattering in a defect-free graphene lattice in resonance with the plasmon. We propose a quantum theory of plasmon-enhanced Raman scattering, where the plasmon forms an integral part of the excitation process. Quantum interferences between scatte…
This study investigated spectral changes in the absorption cross-sections of single strong coupling systems composed of single silver nanoparticle dimers and a few dye molecules during the quenching of surface-enhanced resonant Raman scattering (SERRS). The absorption cross-section was obtained by subtracting the scattering cross-section from an extinction cross-section. The spectral changes in these cross-sections were evaluated using a classical hybridization model composed of a plasmon and a molecular exciton including a molecular multi-level property. The changes in the scattering and exti…
We report on measurements of visible extinction spectra of semicontinuous silver nanoshells grown on colloidal silica spheres. We find that thin, fractal shells below the percolation threshold exhibit geometrically tunable plasmon resonances. A modified scaling theory approach is used to model the dielectric response of such shells, which is then utilized to obtain the extinction cross section in a retarded Mie scattering formalism. We show that such spherical resonators support unique plasmon dynamics: in the visible there is a new regime of coherently driven cluster-localized plasmons, while…
Stimulated Raman scattering (SRS) microscopy allows for high-speed label-free chemical imaging of biomedical systems. The imaging sensitivity of SRS microscopy is limited to ~10 mM for endogenous biomolecules. Electronic pre-resonant SRS allows detection of sub-micromolar chromophores. However, label-free SRS detection of single biomolecules having extremely small Raman cross-sections (~10-30 cm2 sr-1) remains unreachable. Here, we demonstrate plasmon-enhanced stimulated Raman scattering (PESRS) microscopy with single-molecule detection sensitivity. Incorporating pico-Joule laser excitation, b…
We demonstrate that plasmons in graphene can be manipulated using a DC current. A source-drain current lifts the forward/backward degeneracy of the plasmons, creating two modes with different propagation properties parallel and antiparallel to the current. We show that the propagation length of the plasmon propagating parallel to the drift current is enhanced, while the propagation length for the antiparallel plasmon is suppressed. We also investigate the scattering of light off graphene due to the plasmons in a periodic dielectric environment and we find that the plasmon resonance separates i…
The construction of the unconditionally stable planar rank 2 scattering matrix for stratified systems is detailed from Fresnel equations. Several matrix decompositions and numerical calculations performed on the planar S matrix allow for the expedient characterization of purely absorbing, brewster, surface plasmon, and wave-guide modes. A figure of merit is presented from the decompositions of the scattering matrix constructed from the Chandezon method for corrugated surfaces. This figure of merit represents the hyper-area of the scattering matrix transform and allows for rapid distinguishabil…
We investigate the far-field optical resonances of individual dimer nanoantennas using confocal scattering spectroscopy. Experiments on a single-antenna array with varying arm lengths and interparticle gap sizes show large spectral shifts of the plasmon modes due to a combination of geometrical resonances and plasmon hybridization. All resonances are considerably broadened compared to those of small nanorods in the quasistatic limit, which we attribute to a greatly enhanced radiative damping of the antenna modes. The scattering spectra are compared with rigorous model calculations that demonst…
The propagation of a surface plasmon-polariton along a stack of doped graphene sheets is considered. This auxiliary problem is used to discuss: (i) the scattering of such a mode at an interface between the stack and the vacuum; (ii) the scattering at an interface where there is a sudden change of the electronic doping. The formalism is then extended to the {\it barrier problem}. In this system rich physics is found for the plasmonic mode, showing: total reflection, total transmission, Fabry-Pérot oscillations, and coupling to photonic modes.
We discuss the scattering of graphene surface plasmon-polaritons (SPPs) at an interface between two semi-infinite graphene sheets with different doping levels and/or different underlying dielectric substrates. We take into account retardation effects and the emission of free radiation in the scattering process. We derive approximate analytic expressions for the reflection and the transmission coefficients of the SPPs as well as the same quantities for the emitted free radiation. We show that the scattering problem can be recast as a Fredholm equation of the second kind. Such equation can then …
We introduce the quantum mechanical formalism for treating surface plasmon polariton scattering at an interface. Our developed theory - which is fundamentally different from the analogous photonic scenario - is used to investigate the possibility of plasmonic beamsplitters at the quantum level. Remarkably, we find that a wide-range of splitting ratios can be reached. As an application, we characterize a 50:50 plasmonic beamsplitter and investigate first-order quantum interference of surface plasmon polaritons. The results of this theoretical study show that surface plasmon beamsplitters are ab…
We present a theoretical analysis of light scattering from a layered metal-dielectric microsphere. The system consists of two spherical resonators, coupled through concentric embedding. Solving for the modes of this system we find that near an avoided crossing the scattering cross section is dramatically suppressed, exhibiting a tunable optical transparency. Similar to electromagnetically induced transparency, this phenomenon is associated with a large group delay, which in our system is manifest as flat azimuthal dispersion.
We develop a quantum-mechanical theory for Landau damping of surface plasmons in metal nanostructures larger that the characteristic length for nonlocal effects. We show that the electron surface scattering, which facilitates plasmon decay in small nanostructures, can be incorporated into the metal dielectric function on par with phonon and impurity scattering. The derived surface scattering rate is determined by the plasmon local field polarization relative to the metal-dielectric interface and is highly sensitive to the system geometry. We illustrate our model by providing analytical results…
Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of \textit{phonon-stimulated Raman scattering} and an counter-intuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this novel QED framework opens a venue to a…
A scheme of THz radiation using two moderately intense lasers and a moderately relativistic electron beam is proposed. In the scheme, a laser encounters a co-propagating relativistic electron beam, and excites plasmons via the two-plasmon decay. The excited plasmons will emit the THz radiations, interacting with the second laser via the Raman scattering. Our estimation suggests that the mena-free-path of the pump laser to the THz radiation is much shorter than the Thomson scattering. The physical parametes for practical interests are presented.
For the purpose of using plasmonics in an integrated scheme where single emitters can be probed efficiently, we experimentally and theoretically study the scattering properties of single nano-rod gold antennas as well as antenna arrays placed on one-dimensional dielectric silicon nitride waveguides. Using real space and Fourier microscopy correlated with waveguide transmission measurements, we quantify the spectral properties, absolute strength and directivity of scattering. The scattering processes can be well understood in the framework of the physics of dipolar objects placed on a planar la…
The scattering of surface plasmons polaritons by a one-dimensional defect of the surface is theoretically studied, by means of both Rayleigh and modal expansions. The considered defects are either relief perturbations or variations in the permittivity of the metal. The dependence of transmission, reflection and out-of-plane scattering on parameters defining the defect is presented. We find that the radiated energy is forwardly directed (with respect to the surface plasmon propagation) in the case of an impedance defect. However, for relief defects, the radiated energy may be directed into back…
Scattering processes have played a crucial role in the development of quantum theory. In the field of optics, scattering phase shifts have been utilized to unveil interesting forms of light-matter interactions. Here, we investigate the mode-coupling phase of single photons to surface plasmon polaritons in a quantum plasmonic tritter. We observe that the coupling process induces a phase jump that occurs when photons scatter into surface plasmons and vice versa. This interesting coupling phase dynamics is of particular relevance for quantum plasmonic experiments. Furthermore, it is demonstrated …
A scheme of soft-xray radiation is proposed. In the scheme, a moderately intense laser excites plasmons via the two-plasmon decay in a relativistic electron beam. As the second laser encounters the electron beam in the opposite direction, it emits soft x-rays via the backward Raman scattering. Our analysis suggests that the effective cross-section of this scattering is higher than the Thomson scattering and that the conversion efficiency from the pump laser to the soft x-ray could be very high in the optimal scenario. USing the plasmon pump with duration of 1-100 pico-second and the electron b…
In this letter, we study the scattering of light by a single subwavelength slit in a metal screen. In contrast to previous theoretical works, we provide a microscopic description of the scattering process by emphasizing the generation of surface plasmons at the slit apertures. The analysis is supported by a rigorous formalism based on a normal-mode-decomposition technique and by a semi-analytical model which provides accurate formulae for the plasmonic generation strengths. The generation is shown to be fairly efficient for metals with a low conductivity, like gold in the visible regime. Verif…
We map the complex electric fields associated with the scattering of surface plasmon polaritons by single sub-wavelength holes of different sizes in thick gold films. We identify and quantify the different modes associated with this event, including a radial surface wave with an angularly isotropic amplitude. This wave is shown to arise from the out-of-plane electric dipole induced in the hole, and we quantify the corresponding polarizability, which is in excellent agreement with electromagnetic theory. Time-resolved measurements reveal a time-delay of 38? +/- 18 fs between the surface plasmon…
Label free tracking of small bio-particles such as proteins or viruses is of great utility in the study of biological processes, however such experiments are frequently hindered by weak signal strengths and a susceptibility to scattering impurities. To overcome these problems we here propose a novel technique leveraging the enhanced sensitivity of both interferometric detection and the strong field confinement of surface plasmons. Specifically, we show that interference between the field scattered by an analyte particle and a speckle reference field, derived from random scattering of surface p…
The collective excitation of the conduction electrons in subwavelength structures gives rise to the Localized Surface Plasmon(LSP). The system consisting of two such LSPs, known as the dimer system,is of fundamental interest and is being actively investigated in the literature. Three regimes have been previously identified and they are the photonic regime, the strong coupling regime and the quantum tunneling regime. In this Letter, we propose a new regime for this intriguing systems, the intermediate regime. In this new regime, the quasistatic approximation, which is widely used to study such …
Plasmon-enhanced Raman scattering (PERS) becomes nonlinear when phonon pumping and phonon-stimulated scattering come into play. It is fundamental to the understanding of PERS and its photobleaching behavior. By quantization of the molecular vibration coherent state into phonon number states, we theoretically predict a stepwise dependence of PERS intensity on laser power. Experimental evidence is presented by measuring a monolayer of malachite green isothiocyanate molecules sandwiched in individual gold nanosphere-plane antennas, under radially polarized laser excitation of sub-microWatt powers…
We investigate theoretically the optical properties associated to plasmon resonances of metal nanowires with cross section given by low-order Chebyshev nanoparticles (like rounded-tip nanostars or nanoflowers). The impact of the nanoflower shape is analyzed for varying symmetry and deformation parameter through the spectral dependence of resonances, and their corresponding near field distributions. Large field intensity enhancements are obtained at the gaps between petals, apart from the tips themselves, which make these nanostars/nanoflowers specially suitable to host molecules for SERS sensi…
Methods to increase the light scattered from small particles can help improve the sensitivity of many sensing techniques. Here, we investigate the role multiple scattering plays in perturbing the scattered signal when a particle is added to a random scattering environment. Three enhancement factors, parametrising the effect of different classes of multiple scattering trajectories on the field perturbation, are introduced and their mean amplitudes explored numerically in the context of surface plasmon polariton scattering. We demonstrate that there exists an optimum scatterer density at which t…
Nanometer-sized metal particles exhibit broadening of the localized surface plasmon resonance (LSPR) in comparison to its value predicted by the classical Mie theory. Using our model for the LSPR dependence on non-local surface screening and size quantization, we quantitatively relate the observed plasmon width to the nanoparticle radius $R$ and the permittivity of the surrounding medium $ε_m$. For Ag nanospheres larger than 8 nm only the non-local dynamical effects occurring at the surface are important and, up to a diameter of 25 nm, dominate over the bulk scattering mechanism. Qualitatively…
The hybrid Stimulated Raman Scattering - Two Plasmon Decay instability had shown to play the dominant role for plasma waves excitation and energy absorption at interaction of very intense femtosecond obliquely incident $p$-polarized laser pulse (intensity $10^{17}-5\cdot10^{19}$ W/cm$^2$) with a steep gradient ($L\sim λ$) plasma near the quarter critical surface, i.e. within the typical for modern experiments conditions. The plasmons are excited as two wave packets confined near this surface with very wide $\approx ω_0/c$ spatial spectra along its normal. Hence, phase matching conditions for 3…
Metamaterial approach is capable of drastically increasing the critical temperature, Tc, of composite metal-dielectric superconductors. Tripling of Tc was observed in bulk Al-Al2O3 core-shell metamaterials. A theoretical model based on the Maxwell-Garnett approximation provides a microscopic explanation of this effect in terms of electron-electron pairing mediated by a hybrid plasmon-phonon excitation. We report the first observation of this excitation in Al-Al2O3 core-shell metamaterials using inelastic neutron scattering. This result provides support for this novel mechanism of superconducti…
We present a microscopic model describing the transition to strong coupling regime for an emitter resonantly coupled to a surface plasmon in a metal-dielectric structure. We demonstrate that the shape of scattering spectra is determined by an interplay of two distinct mechanisms. First is the near-field coupling between the emitter and the plasmon mode which underpins energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra prior the transition to strong coupling regime. The second mechanism is Fano interference between the plas…
The scattering of light and surface plasmon polaritons (SPPs) by finite arrays of either holes or dimples in a metal film is treated theoretically. A modal expansion formalism, capable of handling real metals with up to thousands of indentations, is presented. Computations based on this method demonstrate that a single hole scatters a significant fraction of incoming light into SPPs. It is also observed that holes and dimples scatter SPPs into light with similar efficiencies, provided the depth of the dimple is larger than its radius. Finally, it is shown that in arrays the normalized-to-area …
Single-molecule surface enhanced Raman scattering (SM-SERS) is one of the vital applications of plasmonic nanoparticles. The SM-SERS sensitivity critically depends on plasmonic hot-spots created at the vicinity of such nanoparticles. In conventional fluid-phase SM-SERS experiments, plasmonic hot-spots are facilitated by chemical aggregation of nanoparticles. Such aggregation is usually irreversible, and hence, nanoparticles cannot be re-dispersed in the fluid for further use. Here, we show how to combine SM-SERS with plasmon-polariton assisted, reversible assembly of plasmonic nanoparticles at…
The conventional explanation of plasmon-enhanced Raman scattering attributes the enhancement to the antenna effect focusing the electromagnetic field into sub-wavelength volumes. Here we introduce a new model that additionally accounts for the dynamical and coherent nature of the plasmon-molecule interaction and thereby reveals an enhancement mechanism not contemplated before: dynamical backaction amplification of molecular vibrations. We first map the problem onto the canonical model of cavity optomechanics, in which the molecular vibration and the plasmon are \textit{parametrically coupled}.…
We explore the far-field scattering properties of anisotropic 2D materials in ribbon array configuration. Our study reveals the plasmon-enhanced linear birefringence in these ultrathin metasurfaces, where linearly polarized incident light can be scattered into its orthogonal polarization or be converted into circular polarized light. We found wide modulation in both amplitude and phase of the scattered light via tuning the operating frequency or material's anisotropy and develop models to explain the observed scattering behavior.
The detailed understanding of the physical parameters that determine Localized Surface Plasmon Resonances (LSPRs) is essential to develop new applications for plasmonics. A relatively new area of research has been opened by the identification of LSPRs in low carrier density systems obtained by doping semiconductor quantum dots. We investigate theoretically how diffuse surface scattering of electrons in combination with the effect of quantization due to size (QSE) impact the evolution of the LSPRs with the size of these nanosystems. Two key parameters are the length $R_0$ giving the strength of…
Electromagnetic coupling between subradiant plasmons and dye molecular excitons analyzed by spectral changes in ultrafast surface-enhanced fluorescence
Health and Medical Research Institute, National Institute of Advanced Industrial Science and Technology (AIST)（产业技术综合研究所健康与医学研究所）；School of Materials Science, Japan Advanced Institute of Science and Technology (JAIST)（日本高级科学技术研究院材料科学学院）
